Issue 35, 2024

Resolving local ordering and structure in MnxGe1−xTe alloys through thermodynamic ensembles of pair distribution functions

Abstract

Characterizing local bonding environments in complex materials is essential for understanding and optimizing their properties. Equally as important is the ability to predict local motifs as a function of synthesis conditions, enhancing chemists’ ability to design properties into materials. In this study, we present an approach to leverage statistical mechanics to generate temperature- and energy-informed ensemble averaged pair distribution functions (PDFs). This method, which we have named Thermodynamic Ensemble Averages of PDFs for Ordering and Transformations (TEAPOT), utilizes density functional theory (DFT) to relax supercells while incorporating energetic penalties for local order, enabling accurate and computationally efficient analysis of local structure. We apply this method to the neutron PDF measurements of the pseudobinary MnTe–GeTe (MGT) alloy, demonstrating its capability to resolve complex local distortions and chemical ordering. Our results reveal detailed insights into phase transformations and local distortions driven by Mn substitution. For compositions that globally present as rock salt, our analysis reveals that Ge coordination geometry is heavily impacted by synthesis temperature. We propose that high temperature synthesis conditions promote a lowered Ge polyhedra distortion, promoting high charge carrier mobility due to the alignment of local and global structure. Incorporating statistical mechanics and computation into experimental analysis thus guides synthesis of tailored local structure.

Graphical abstract: Resolving local ordering and structure in MnxGe1−xTe alloys through thermodynamic ensembles of pair distribution functions

Supplementary files

Article information

Article type
Paper
Submitted
09 jul. 2024
Accepted
02 ago. 2024
First published
02 ago. 2024
This article is Open Access
Creative Commons BY-NC license

J. Mater. Chem. C, 2024,12, 13863-13874

Resolving local ordering and structure in MnxGe1−xTe alloys through thermodynamic ensembles of pair distribution functions

V. Meschke, A. Novick, J. Rogers, C. Porter, R. Chang, T. Proffen and E. S. Toberer, J. Mater. Chem. C, 2024, 12, 13863 DOI: 10.1039/D4TC02896A

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